Biocomposites exhibit properties like many petrochemical-based polymers composites. They have the potentials be used in the automotive and decking industries and as biodegradable packaging. However, the high cost as well as, poor mechanical and thermal properties have restricted their widespread use. There are a number of technical issues that need to be addressed before bio-composites can be widely used.
In this research Polylactic acid (PLA) composites, reinforced with natural fibres (wood, flax) and mineral fillers (talc) were investigated. The thermal and mechanical properties of the composites were studied by means of Differential Scanning Calorimetry (DSC), Tensile Testing and Dynamic Mechanical Analysis (DMA), while morphology and crystallization processes of the composites were studied by hot stage optical microscopy. The experimental results are also compared with different theoretical models of the response of the composites.
PLA / wood composites were developed by mixing PLA with wood in different ratios using a melt compounding process. PLA/wood (90/10. 80/20, 60/40), PLA/wood/copolymers (85/10/05, 80/10/10, 75/20/05, 70/20/10, 55/40/05, 50/40/10) and PLA/wood/coupling agent (80/20/silane coating) were the three different composite systems that were developed. Adding increasing amount of wood into the PLA, the thermal properties remain unchanged but the mechanical properties increased significantly, bringing a stiffening effect to the composites. Tensile modulus increased from 4.1± 0.6 to 9.8 ± 1.2 (GPa) as the wood content increased from 0 to 40 (wt %), but the tensile strength at break reduced from 43.8 ± 3.1 to 31.8 ± 2.8 MPa. The experimental results of the PLA-wood composites were modelled according to the Halpin-Tsai equation.
The addition of copolymer affected the thermal properties considerably by decreasing the glass transition temperature of the composite. The glass transition temperature dropped from 54 ± 0.7 (0C) to 48 ± 0.36 (0C) when the content of copolymer was increased from 0 to 10 (wt %). The cold crystallization temperature also decreased from 127 ± 1.41 (0C) to 103 ± 2.58 (0C) when the copolymer was incorporated into the PLA/wood composites. The significant aspect was the occurrence of a double peak in the melting endotherm. The degree of crystallinity also increased from 2 ± 0.83 (%) to 11 ± 1.23 (%) when the amount of copolymer was increased to 10 (wt %).
PLA, flax and expoidizied natural rubber (ENR) composites were also developed using a melt compounding process. The mechanical properties were affected significantly when the flax fibres were mixed with PLA in the ratios of 10, 20 and 30 (wt %). Addition of flax fibres increased the elastic modulus significantly but reduced the tensile strength and strain at break. To improve the toughness of the PLA- Flax composites, ENR was incorporated into the PLA- Flax composites.
In order to balance the modulus of the reinforcement and the matrix, the PLA- Flax and ENR composites were annealed above the glass transition temperature and the degree of crystallinity increased from 2 to 35 (%). The integral blending of PLA, Flax and ENR did not affect the brittle fracture but introducing a masterbatch of flax fibres and ENR into the PLA matrix during melt processing had a considerable effect on the fracture behaviour of the composites. The elastic modulus of the composites decreased due to the elastomeric content in the composites and there was an increase in elongation-to-break.
The effect of talc on the crystallinity and mechanical properties of a series of polylactic acid (PLA) / talc composites was investigated. PLA talc composites were developed by incorporating different types of the talc into the PLA in the ratios of 10, 20 and 30 (wt %). The composites were prepared by melt blending followed by compression moulding. It was found that talc acted as a nucleating agent and increased the crystallinity of the PLA from 2% to 25%. There was significant improvement in Young s modulus of the composites with increasing talc addition and these results were found to fit the Halpin Tsai model. Thermo-mechanical tests confirmed that the combination of increased crystallinity and storage modulus leads to improvement in the heat distortion properties.

Description:

A Doctoral Thesis. Submitted in partial fulfilment of the requirements for the award of Doctor of Philosophy of Loughborough University.